ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Jingjiao Cao,Wanjian Shan,Qian Wang,Xingchen Ling,Guoqing Li,Yinong Lyu,Yu Zhou,Jun Wang
Porous poly(ionic liquid)s (PPILs) combine the features of porous materials, polymers, and ionic liquids (ILs) or their derivatives, but they are normally of amorphous structure with disordered pores. Here, we report the facile synthesis of ordered porous poly(ionic liquid) crystallines (OPICs, specialized as a kind of PPIL analogues) with diverse and adjustable framework IL moieties through the Schiff base condensation of IL-derived ionic salts and neutral monomers. Ternary monomer mixtures are employed to artistically control the chemical composition and pore configurations. Compact atomic packing was achieved to give spacing confined ionic surface with strong CO2 affinity. Through monomer control, OPICs exhibit high CO2 uptakes with excellent CO2/N2(CH4) selectivities and efficiently implement CO2 fixation through catalyzing epoxides cycloaddition under down to ambient conditions.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED ENERGY
·
2019
·
IF 8.426
Zhen-Feng Sun,Nan Li,Shuai Jia,Jin-Long Cui,Qing Yuan,Chang-Yu Sun,Guang-Jin Chen
To enhance the exploitation efficiency of natural gas hydrate by decreasing the yield of water, a novel “reservoir reformation” concept is proposed that involves the reformation of a natural gas hydrate reservoir by constructing an artificial impermeable overlying CO 2 hydrate cap. The feasibility of this concept has been demonstrated in this laboratory-scale experiment. After reformation by injecting CO 2 emulsion into the permeable overburden, a confined environment with an impermeable CO 2 hydrate cap is successfully constructed for depressurization operation. The cap can maintain mechanical stability until the end of production process. With the protection provided by the artificial CO 2 hydrate cap, the production efficiency was greatly improved to 83.3% and the water yield is remarkably decreased. Moreover, the optimal CO 2 /H 2 O volume ratio of the emulsion for forming the desired CO 2 hydrate cap was confirmed to be 1:1. The formation of CO 2 hydrate cap can also protect the geological stability of depleted methane hydrate zones and seal a large amount of CO 2 , which is of both energetic and environmental significance; however, intensive and extensive research should be conducted in the future.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2019
·
IF 3.571
Sizhu Ren,Conghai Li,Zhilei Tan,Ying Hou,Shiru Jia,Jiandong Cui
In this study, carbonic anhydrase (CA, EC 4.2.1.1) molecules were embedded into metal–organic frameworks (MOFs) via co-precipitation (CA@ZIF-8), and then these CA@ZIF-8 nanocomposites were encapsulated in the poly(vinyl alcohol) (PVA)–chitosan (CS) hydrogel networks to prepare CA@ZIF-8–PVA–CS composite hydrogels (PVA/CS/CA@ZIF-8) with high activity, stability, and reusability. The immobilization efficiency of CA was greater than 70%, suggesting the high immobilization efficiency. The prepared PVA/CS/CA@ZIF-8 composite membranes displayed excellent higher stability against a high temperature, denaturants, and acid than free CA and CA@ZIF-8. Furthermore, these membranes exhibited an excellent performance for CO2 capture. The amount of calcium carbonate obtained by PVA/CS/CA@ZIF-8 hydrogel membranes was 20- and 1.63-fold than free CA and CA@ZIF-8 composites, respectively. Furthermore, the hydrogel membranes exhibited superior reusability and mechanical strength. The hydrogel membrane maitained 50% of its original activity after 11 cycles. However, CA@ZIF-8 completely lost activity. These results indicated that the PVA/CS/CA@ZIF-8 membranes can be efficiently applied to capture CO2 sequestration.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Junjie Zhu,Linbo Wu,Zhiyang Bu,Suyun Jie,Bo-Geng Li
Searching for highly efficient and robust CO2 adsorbents is very important for CO2 capture, utilization, and storage. In this study, new polyethylenimine-grafted metal–organic framework (MOF)–polymer composites, abbreviated as PEI@PGD-H, were synthesized via high internal phase emulsion (HIPE) template polymerization of divinylbenzene and glycidyl methacrylate, followed by in situ generation of HKUST-type MOF in the presence of hydrophobic-modified CuO nanoparticles via the reaction of CuO with 1,3,5-benzenetricarboxylic acid and then polyethylenimine (PEI) functionalization via epoxy–amine reaction and amine–metal sites interaction. The coexistence of the hierarchical interconnected porous skeleton of poly(glycidyl methacrylate–divinylbenzene) (PGD), high specific surface area of MOF, and chemical CO2 adsorption of PEI endows PEI@PGD-H with high CO2 adsorption capacity, rate, and selectivity. PEI70@PGD-H shows a CO2/N2 separation factor as high as 76 and CO2 adsorption capacities of 4.3, 3.0, and 1.8 mmol of CO2/g from pure CO2, simulated flue gas, and air, respectively. After 20 CO2 adsorption–desorption cycles, the adsorbent still retained a high and stable CO2 capture capacity over 2.8 mmol of CO2/g for simulated flue gas. The adsorbent also displays reasonably good thermal stability, excellent water endurance, low desorption energy, and easy shaping. The desorption heat is as low as 48 kJ/mol of CO2. These features make PEI@PGD-H highly efficient, robust, and low-energy CO2 adsorbents for practical application in CO2 capture.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Rongrong He,Shenzhen Cong,Jing Wang,Jindun Liu,Yatao Zhang
The computational simulation of porous graphene oxide (PGO) indicated that it has great potential for the preparation of gas separation membranes. However, scaling up the manufacture of multilayer, defect-free porous graphene oxide membrane with consistently sized nanopores is extremely challenging. Here, we prepared layer-by-layer CO2-philic Pebax@1657 membranes that were functionalized by o-hydroxyazo-hierarchical porous organic polymers (o-POPs) and PGO. The d-spacing of pristine PGO could be finely regulated through CO2-philic o-POPs to facilitate the permeability of CO2. In addition, the o-POPs exhibit “N2-phobic, CO2-philic” properties with the phenolic hydroxyl and the azo group. The best of the POP-PGO membrane exhibits that the CO2 permeability and ideal selectivity of CO2/N2 are 232.7 Barrer and 80.7, respectively, and it has surpassed the Robeson’s upper bound (2008).
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2019
·
IF 5.128
Shuang Yue,Pingping Wang,Xueying Hao
The bifunctional imidazolium ionic liquids ([HEMim][Glu], [HEMim][Asp], [HEBim][Asp], [HEBim][Ala], [HEBim][His]) were successfully synthesized and characterized by 1 H NMR, 13 C NMR, COSY, HSQC and FT-IR spectroscopy. The ionic liquids performed as bifunctional catalysts and exhibited high catalytic activity for the cyclic carbonate synthesis from CO 2 and epoxides under mild conditions with excellent yields in the absence of any solvents or co-catalysts. The reaction time, reaction temperature, CO 2 pressure and the amount of ionic liquid were systematically investigated. The catalyst can be reused for at least four cycles without any significant drop in the catalyst activity and hence represents a reasonably environmentally benign chemical process for CO 2 fixation.
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2019
·
IF 2.938
Qingshuo Li,Haibo Chang,Runming Li,Hongxia Wang,Jichun Liu,Shanhu Liu,Congzhen Qiao,Tong Lin
In this study, we have for the first time demonstrated that succinimide (SI)-KI is an efficient catalyst system to synthesize propylene carbonate (PC) from carbon dioxide (CO 2 ) and propylene oxide (PO) at a solvent-free condition. A synergistic effect was observed between SI and KI that largely increased the reaction yield. It enabled the cycloaddition reaction to take place at 70 °C under a low pressure (0.4 MPa) for only 4 h, with a PC yield as high as 97.5%. The overall condition is milder than the reaction catalyzed by most of the other KI involved co-catalyst systems reported in literatures. The excellent catalytic ability was explained by the increased KI solubility in PO due to the presence of SI and the weak acidity of NH in SI which can be enhanced by KI. A reaction mechanism was proposed based on a reaction kinetics study. SI-KI was applicable to cycloaddition of CO 2 with other epoxides. It may offer an inexpensive, environmentally-friendly route to synthesis of propylene carbonate from CO 2 .
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2019
·
IF 7.466
Chao Hu,Ye Mu,Silin Bai,Juan Yang,Lijun Gao,Shao-Dong Cheng,Shao-Bo Mi,Jieshan Qiu
Electrochemically converting CO 2 into fuels or high value-added chemicals hold a great promise for the utilization of emitted CO 2 in the future. Metal-nitrogen active sites (such as Fe–N, Co–N and Ni–N) are supposed to be effective for the electrochemical reduction of CO 2 to CO, whereas their catalytic activities are largely dependent on the dispersibility and bonding structures of the catalytically active metals. In this work, we develop atomically dispersed Fe, N-codoped sandwich-like porous carbon sheets using Fe-containing zeolitic imidazolate framework-8 and graphene oxide as precursors and polyvinyl pyrrolidone (PVP) as a mediator. Compared to catalysts without PVP or with another mediator (i.e. polyetherimide), the PVP-mediated carbon sheets show a porous morphology with a higher specific surface area and a more exposed number of Fe–N active sites. Benefiting from this favourable structure, the resultant Fe, N-codoped porous carbon sheets show higher current densities and improved faradaic efficiencies up to 98.6% at −0.62 V ( vs. the reversible hydrogen electrode, RHE) for the electrochemical reduction of CO 2 to CO. This PVP-mediated strategy could be applied to the fabrication of other metal/nitrogen codoped carbon materials for electrocatalysis.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Hengxuan Zhao,Yuefei Ji,Deyang Kong,Junhe Lu,Xiaoming Yin,Quansuo Zhou
Iodinated X-ray contrast media (ICM) are a group of tri-iodinated aromatic compounds used in medical imaging of soft tissues. They are regarded as emerging contaminants , and widely detected in the effluents of wastewater treatment plants , surface water, and groundwater. In the present study, degradation of iohexol, a typical ICM agent, was systematically investigated in a Co 2+ activated peroxymonosulfate (Co 2+ /PMS) oxidation process at neutral conditions. Experimental data revealed that the apparent rate of iohexol degradation was first-order with respect to the concentrations of both Co 2+ and PMS. SO 4 − was found to induce the oxidative degradation of iohexol primarily. Presence of humic acid (HA) significantly inhibited the iohexol degradation, while the influence of Cl − was negligible. A total of 11 intermediates were identified by HPLC-MS/MS and three transformation pathways, i.e., cleavage of side chain, H-abstraction from side chain, and oxidative deiodination, were proposed. The degradation started with the oxidation of the side chains in iohexol molecule and followed by deiodination on the aromatic ring. Following the degradation of iohexol, formation of free iodine and iodinated disinfection byproducts (I-DBPs) was found. When 50 µM was treated with 1 mM PMS and 1 µM Co 2+ , the yields of iodoform and triiodoacetic acid reached 38.12 and 577.99 µg/L, respectively, in 12 h. In addition, the formation of I-DBPs was prominently enhanced by the presence of HA. Because I-DBPs are highly toxic, this study suggests the potential risks when SO 4 − is applied to degrade ICM compounds.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Jiawen Liao,Bo Jin,Yunlei Zhao,Zhiwu Liang
Calcium looping is a promising technology for CO 2 capture, although traditional calcium-based sorbents undergo a rapid loss of capacity after repeated cycles. Improving the toughness of sorbents can be accomplished with the use of stabilizer compounds, but at the cost of sorption performance. Minimizing the stabilizer content whilst maintaining high thermal stability is an effective pathway to solve this bottleneck. Here, a facile MOF-templated synthesis route is for the first time reported to yield highly efficient Al 2 O 3 -stabilized, Ca-based sorbents. Cyclic performance experiments and detailed characterization techniques are employed to identify the effects of synthesis factors on the structure-performance relationship of the synthesized CO 2 sorbents. Calcium aluminum solid solution and its homogeneous mixture with CaO at the nanoscale provide for high thermal stability. The different CO 2 uptake behavior for the synthesized sorbents primarily results from the influence of synthesis factors on the crystallization rates and coordination modes between metal ion and organic ligands. The stabilizer content (i.e. Al 2 O 3 ) can be as low as 4.44 wt% and yet maintain a favorable thermal stability. Compared to that of the limestone-derived CO 2 sorbents, the best MOF-derived sorbent can achieve about 500% times the CO 2 sorption capacity after 30 repeated CO 2 uptakes and sorbent regenerations.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SUPERCRITICAL FLUIDS
·
2019
·
IF 3.481
Ze-Hao Li,Li Wang,Hong-Lian Dai,Xin-Yu Wang,Jia-Shen Li,Zheng Zhao
Scaffolds that mimic the nanofibrous structures of extracellular matrix (ECM) are essential for cell adhesion and proliferation in tissue engineering. In this study, silk fibroin (SF) scaffolds with interconnected porous and ECM-like nanofibrous structures were prepared by successfully combining supercritical CO 2 technology with a porogen leaching process. The effects of pressure and concentration of the SF solution on the nanofibrous structures of the SF scaffolds were not significant. By manipulating the proportion of porogen, SF scaffolds with a porosity of (32.7 ± 1.7) % to (82.1 ± 2.3) % and a mechanical strength of (237.0 ± 2.2) kPa to (163.0 ± 6.5) kPa were fabricated. In vitro biocompatibility evaluation using a MTT assay, DAPI staining, and SEM observation indicated that the SF scaffolds exhibited no toxicity and could facilitate Schwann cell attachment and proliferation. Therefore, the biomimetic SF porous scaffolds with ECM-like nanofibrous structure have potential application in nerve regeneration.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Long Ma,Changlei Qin,Shuai Pi,Henan Cui
Li 4 SiO 4 is a promising solid sorbent for high-temperature CO 2 capture due to the high and stable CO 2 adsorption performance. It is required to possess good mechanical properties in practical fluidized-bed systems and pelletization is necessary. However, pelletization generally results in a large decline in the CO 2 uptake or a continuous loss-in-capacity of Li 4 SiO 4 sorbents in cyclic reactions. In this work, three kinds of Li 4 SiO 4 powders were synthesized and screened, and spherical pellets were further prepared via an extrusion-spheronization technique using polyethylene as a pore-former to develop porous microstructure. Then sorbent pellets were systematically tested on the CO 2 adsorption performance, compression strength and attrition resistance. Results shows that the pellets modifying with 20 wt% polyethylene reach and stabilize a CO 2 sorption capacity of 0.31 g CO 2 /g sorbent in the whole 40 tested cycles under typical conditions, which is even higher than that in powder form. Moreover, the pellets are observed to have an outstanding compression strength (27.5 MPa after calcination) and an excellent attrition resistance (only 1.01 wt% mass loss in 10 h-attrition test), which are both far more better than sorbents reported in the literature. The simultaneous physiochemical performances indicate that the prepared Li 4 SiO 4 sorbent pellets could be suitable for high temperature CO 2 capture in fluidized-bed reactors.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）